The objective of this study was to investigate the rate of mobile phone use among car drivers in Greece and its association with drivers’ characteristics and other parameters. Data collected through an observation survey were used in a binary logistic regression model which highlighted the explanatory factors of using a mobile phone while driving. Pseudo-elasticities quantified the impact of each variable on mobile use. The observation survey showed that 9% of car drivers in Greece use a hand-held mobile phone. The dependent variable with the greatest impact was the driver’s age being between 16 and 24 years. The results will assist the development of targeted intervention strategies to decrease mobile phone use while driving and will act as a baseline against which the effect of these interventions can be measured. Education and information campaigns have a key role in increasing public awareness regarding the risks involved in using a mobile phone in traffic.